For bone tissue engineering, additive manufacturing offers promise in the development of biomimetic scaffolds; however, common polymers used in typical 3D printing methods often suffer from less than ideal surface properties for proper mineralization. As a result, they can underperform with respect to biointegration without additional modification. In this study, low-temperature plasma was utilized to modify the surface of 3D printed poly(lactic acid) (PLA) for promoting mineralization in biomimetic in vitro conditions. Detection of calcium phosphates on the polymer surfaces was accomplished via Fourier transform infrared (FT-IR) spectroscopy and X-ray photoelectron (XPS) spectroscopy. Scanning electron microscopy (SEM) was employed to identify and image the mineralization products on the surfaces of the scaffolds. Further, a fluorescent assay of surface extracts identified calcium-containing mineral deposits at significantly higher levels for treated scaffolds versus controls. Taken together, these results suggest the futuristic potential of this surface modification method for bone tissue engineering applications. Graphical abstract: [Figure not available: see fulltext.]